物理化学学报 >> 2010, Vol. 26 >> Issue (04): 869-876.doi: 10.3866/PKU.WHXB20100441

催化和表面结构 上一篇    下一篇

低温加氢催化剂的设计: 理论与实践

陈经广, 齐随涛, HUMBERT Michael P, MENNING Carl A, 朱月香   

  1. Department of Chemical Engineering, Center for Catalytic Science and Technology (CCST), University of Delaware, Newark, DE 19716, USA; 西安交通大学化工系, 西安 710049; 北京大学化学与分子工程学院, 北京分子科学国家实验室, 分子动态与稳态结构国家重点实验室, 北京 100871
  • 收稿日期:2009-11-30 修回日期:2010-03-07 发布日期:2010-04-02
  • 通讯作者: 陈经广 E-mail:jgchen@udel.edu

Rational Design of Low-Temperature Hydrogenation Catalysts: Theoretical Predictions and Experimental Verification

CHEN Jingguang G, QI Sui-Tao, HUMBERT Michael P, MENNING Carl A, ZHU Yue-Xiang   

  1. Department of Chemical Engineering, Center for Catalytic Science and Technology (CCST), University of Delaware, Newark, DE 19716, USA; Department of Chemical Engineering, Xi'an Jiaotong University, Xi'an 710049, P. R. China; Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, P. R. China
  • Received:2009-11-30 Revised:2010-03-07 Published:2010-04-02
  • Contact: CHEN Jingguang G E-mail:jgchen@udel.edu

摘要:

简要总结了我们在C=C及C=O双键低温加氢双金属催化剂方面的最新研究成果. 首先, 我们以环己烯加氢为探针反应, 证明了平行使用多种研究手段的重要性, 包括单晶表面的基础研究与DFT计算, 多晶表面的合成与表征, 负载型催化剂的制备与性能测试等. 其次, 总结了双金属催化剂在其他加氢反应, 如丙烯醛C=O双键的选择性加氢, 苯的低温加氢, 以及乙炔的选择性加氢等反应中的应用. 最后, 讨论了利用金属碳化物代替贵金属Pt以减少双金属催化剂中Pt用量的可能性.

关键词: 加氢, 双金属催化剂, 金属碳化物, DFT计算

Abstract:

In this review, we will provide a brief review of our recent theoretical and experimental studies of bimetallic surfaces and catalysts for the low-temperature hydrogenation of unsaturated C=C and C=O bonds. We will first use the hydrogenation of cyclohexene as a probe reaction to demonstrate the importance of using several parallel approaches, including fundamental surface science and density functional theory (DFT) studies on single crystal surfaces, synthesis, and characterization of polycrystalline surfaces and supported catalysts, and reactor evaluation of supported catalysts. We will then provide a summary of applications of bimetallic catalysts for other hydrogenation reactions, including the selective hydrogenation of the C=O bond in acrolein, the low-temperature hydrogenation of benzene, and the selective hydrogenation of acetylene in the presence of ethylene. Finally, we will discuss the possibility of replacing the platinum(Pt) component with metal carbides to reduce the loading of Pt in bimetallic catalysts.

Key words: Hydrogenation, Bimetallic catalyst, Metal carbide, Density functional calculation

MSC2000: 

  • O643